A typical nuclear magnetic resonance (NMR) gyroscope operates on the principle of sensing inertial angular rotation rate or orientation angle about a sensitive axis based on a shift in the measured Larmor precession frequency or phase of one or two isotopes that possess nuclear magnetic moments. An NMR gyroscope (“gyro”) system can include a gyro cell and a rotation sensor that includes, for example, a light source, a photodetector, and signal processing circuitry. As an example, the gyro cell can contain one or more alkali metal vapors, such as Rubidium, together with one or more gyromagnetic isotopes that are caused to precess in response to a magnetic field. The signal processing circuitry can extract the Larmor precession frequency and/or phase information of the one or more gyromagnetic isotopes. As a result, a gyroscope rotation rate or orientation angle about the sensitive axis can be calculated based on the extracted Larmor precession frequencies and phase information.